CN111081890A - Phosphorescence-sensitized fluorescent white light organic light-emitting diode and preparation method thereof - Google Patents
Phosphorescence-sensitized fluorescent white light organic light-emitting diode and preparation method thereof Download PDFInfo
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- H10K50/125—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers specially adapted for multicolour light emission, e.g. for emitting white light
- H10K50/13—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers specially adapted for multicolour light emission, e.g. for emitting white light comprising stacked EL layers within one EL unit
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Abstract
The invention belongs to the technical field of organic light emitting diodes, and discloses a phosphorescence-sensitized fluorescent white light organic light emitting diode and a preparation method thereof. The OLEDs structure sequentially comprises a substrate, an anode, a hole injection layer, a hole transport layer, an electron blocking layer, a light emitting layer, an electron transport layer, an electron injection layer and a cathode; the light-emitting layer is formed by combining a blue light-emitting layer and a yellow light-emitting layer, the blue light-emitting layer is formed by doping a blue light phosphorescence sensitizer and a blue light fluorescence object in a host material, and the yellow light-emitting layer is formed by doping a yellow light phosphorescence sensitizer and a yellow light fluorescence object in the host material. The white light OLEDs of the invention adopt a blue light and yellow light double-luminescent-layer structure, and different phosphorescent sensitizers and fluorescent luminescent materials are doped in the main body, so that the high-efficiency full-fluorescent white light OLEDs with wide spectrum coverage and stable spectrum are realized, and a new way is provided for preparing the high-efficiency white light OLEDs.
Description
Technical Field
The invention belongs to the technical field of organic light emitting diodes, and particularly relates to a phosphorescence-sensitized fluorescent white light organic light emitting diode and a preparation method thereof.
Background
Organic Light-Emitting Diodes (OLEDs) are devices based on Organic semiconductors that emit Light under the influence of an electric field. OLEDs have the advantages of high efficiency, lightness, thinness, flexibility, low cost, and large area fabrication, and have wide applications and developments in full color displays and solid state lighting. When OLEDs are used for white light illumination, in order to make the emission spectrum of white light cover the entire visible light region as much as possible and achieve a high Color Rendering Index (CRI), it is usually necessary to combine organic light-emitting materials of multiple colors together through reasonable structural design, such as blue light, green light, and red light three primary colors or two complementary colors of blue light and yellow light, so that the light-emitting materials of different light colors emit light simultaneously, and finally, high-performance white OLEDs are obtained. Therefore, in order to obtain white light OLEDs with good spectrum and high efficiency, it is very important to optimize the material system and design a reasonable device structure.
The all-fluorescent white-light OLEDs have the advantages of low efficiency roll-off, good stability and low cost, and have attracted extensive research and attention. However, according to the spin statistical theory, the conventional fluorescent material only utilizes 25% of singlet excitons to emit light through radiative transition, and 75% of triplet excitons are lost through non-radiative transition, which has a great limitation on improving the efficiency of the fluorescent white OLEDs. Therefore, the key to realizing high-efficiency all-fluorescent white OLEDs is how to use all the generated singlet excitons and triplet excitons for radiative emission. At present, the method of adopting phosphorescence to sensitize fluorescence is considered to be an effective method for preparing high-efficiency fluorescent white light OLEDs, and by introducing a sensitizing agent, triplet exciton energy on sensitizing molecules is effectively transferred to singlet excitons of fluorescent molecules, and all excitons emit light on the fluorescent molecules, so that the utilization rate of the excitons is 100%. However, in the design of the light emitting layer of the phosphorescence-sensitized fluorescent white light OLEDs, the energy levels of the host material, the phosphorescence material and the fluorescent light emitting material need to be effectively matched, and the light emitting layer structures with different light colors need to be reasonably designed to obtain the high-performance all-fluorescent white light OLEDs, so that no significant progress has been made in the adoption of the phosphorescence-sensitized fluorescent white light OLEDs at present.
Disclosure of Invention
Aiming at the defects and shortcomings of the prior art, the invention mainly aims to provide a phosphorescence-sensitized fluorescent white light organic light-emitting diode.
The invention also aims to provide a preparation method of the phosphorescence-sensitized fluorescent white organic light-emitting diode.
The purpose of the invention is realized by the following technical scheme:
a phosphorescence-sensitized fluorescent white organic light-emitting diode structurally comprises a substrate, an anode, a hole injection layer, a hole transport layer, an electron blocking layer, a light-emitting layer, an electron transport layer, an electron injection layer and a cathode in sequence; the light-emitting layer is formed by combining a blue light-emitting layer and a yellow light-emitting layer, the blue light-emitting layer is formed by doping a blue light phosphorescence sensitizer and a blue light fluorescence object in a host material, and the yellow light-emitting layer is formed by doping a yellow light phosphorescence sensitizer and a yellow light fluorescence object in the host material.
Further, the host material of the blue light emitting layer is 26DCzPPy (2, 6-bis ((9H-carbazol-9-yl) -3, 1-phenylene) pyridine), and the blue light phosphorescence sensitizer is fac-Ir (iprpmi)3(tris [1- (2, 6-isopropylbenzene) -2-phenyl-1H-imidazole]Iridium (III)) and the blue-light fluorescent guest is TBPe (1,4,7, 10-tetra-tert-butylphthalene); the host material of the yellow light emitting layer is 26DCzPPy, and the yellow phosphorescent sensitizer is Ir (ppy)3(tris (2-phenylpyridine) iridium (III)) and the yellow fluorescent guest is TBRb (2, 8-di-tert-butyl-5, 11-bis (4-tert-butyl-phenyl) -6, 12-diphenyltetracene).
Further, the blue phosphorescent sensitizer fac-Ir (iprpmi)3The doping concentration of the blue light fluorescent guest TBPe is 8 wt.%, and the doping concentration of the blue light fluorescent guest TBPe is 1 wt.%; yellow phosphorescent sensitizer Ir (ppy)3Has a doping concentration of 6 wt.%, and the yellow fluorescent guest TBRb has a doping concentration of 2 wt.%.
Further, the thickness of the blue light emitting layer is 3-15 nanometers, and the thickness of the yellow light emitting layer is 5-15 nanometers.
Further, the substrate is one of glass, quartz, or flexible plastic.
Further, the anode is one of Indium Tin Oxide (ITO), zinc oxide (ZnO), fluorine-doped tin dioxide (FTO) or graphene.
Further, the hole injection layer can adopt an organic material HAT-CN (2,3,6,7,10, 11-hexacyano-1, 4,5,8,9, 2-azabenzophenanthrene) or an inorganic material MoO3(molybdenum oxide), WO3(tungsten oxide) or V2O5(vanadium pentoxide).
Further, the hole transport layer is preferably TAPC (4, 4' -cyclohexylbis [ N, N-bis (4-methylphenyl) aniline ]).
Further, the electron blocking layer is preferably TCTA (4, 4', 4 ″ -tris (carbazol-9-yl) triphenylamine).
Further, the electron transport layer is preferably TmPyPB (3,3 '- [ 5' - [3- (3-pyridyl) phenyl ] [1,1 ': 3', 1 '-terphenyl ] -3, 3' -diyl ] bipyridine).
Further, the electron injection layer may employ LiF (lithium fluoride), Liq (lithium octahydroxyquinoline), Li2CO3(lithium carbonate) or Cs2CO3(cesium carbonate).
Further, the cathode is made of one of gold (Au), silver (Ag), aluminum (Al) or silver-magnesium alloy.
Furthermore, the thickness of the hole injection layer is 5-20 nanometers, the thickness of the hole transmission layer is 50-90 nanometers, the thickness of the electron blocking layer is 5-15 nanometers, the thickness of the light emitting layer is 15-30 nanometers, the thickness of the electron transmission layer is 40-80 nanometers, the thickness of the electron injection layer is 1-5 nanometers, and the thickness of the cathode is 100-200 nanometers.
The preparation method of the phosphorescence-sensitized fluorescent white organic light-emitting diode comprises the following steps: firstly, carrying out ultrasonic treatment, deionized water flushing, nitrogen blow-drying, baking in a 120 ℃ oven, carrying out ultraviolet ozone treatment on the surface of the ITO glass, then putting the ITO glass into a vacuum coating machine, and vacuumizing by using a molecular pump until the pressure is 8 multiplied by 10-5After Pa is below, sequentially evaporating a hole injection layer, a hole transport layer, an electron blocking layer, a luminescent layer, an electron transport layer, an electron injection layer and a cathode to obtain the phosphorescence-sensitized fluorescent white light organic compoundAn organic light emitting diode.
The principle of the invention is as follows: the blue light emitting layer and the yellow light emitting layer are in a double-layer structure, the two light emitting layers are doped in a main material by different phosphorescent sensitizers and fluorescent materials respectively, triplet excitons are utilized by utilizing the orbital coupling effect of the phosphorescent materials, and the generated singlet excitons and triplet excitons are transferred to the fluorescent materials to emit light by radiation. The full-fluorescence white-light OLEDs with high efficiency, low roll-off and stable spectrum are prepared by the effective matching of the energy levels of the main body, the phosphorescent sensitizer and the fluorescent material and the structural design of the thickness and the position of the blue light emitting layer and the yellow light emitting layer.
Compared with the prior art, the invention has the following advantages and beneficial effects:
(1) the white light OLEDs related to the invention adopt the mode of sensitizing the fluorescent material by the phosphorescent material, and transfer the energy of triplet excitons of the phosphorescent material to the singlet state of the fluorescent luminescent material, thereby realizing 100 percent of exciton utilization rate and leading the prepared white light OLEDs to have the characteristics of high efficiency and low roll-off.
(2) The white light OLEDs related to the invention adopt a blue light and yellow light double-emitting layer structure, the blue light emitting layer and the yellow light emitting layer are respectively doped in a main body by adopting different phosphorescent sensitizers and different fluorescent light emitting materials, and the thickness and the position of the blue light emitting layer and the yellow light emitting layer are adjusted by optimizing the doping concentration, so that the high-efficiency full-fluorescent white light OLEDs with wide spectrum coverage and stable spectrum are realized, and a new way is provided for preparing high-efficiency white light OLEDs.
Drawings
FIG. 1 is a schematic view showing the structure of a phosphorescent-sensitized fluorescent white light OLEDs (W1) according to example 1 of the present invention. Wherein 1 represents a substrate, 2 represents an anode, 3 represents a hole injection layer, 4 represents a hole transport layer, 5 represents an electron blocking layer, 6 represents a yellow light emitting layer, 7 represents a blue light emitting layer, 8 represents an electron transport layer, 9 represents an electron injection layer, and 10 represents a cathode.
FIG. 2 is a graph showing current efficiency, power efficiency and external quantum efficiency-luminance characteristics of phosphorescent-sensitized fluorescent OLEDs (W1) obtained in example 1 of the present invention.
FIG. 3 shows that the phosphorescence-sensitized fluorescent white light OLEDs (W1) obtained in example 1 of the present invention are 1000cd/m2、3000cd/m2And 5000cd/m2Electroluminescence spectrum at brightness.
FIG. 4 is a graph showing current density-luminance-voltage characteristics of phosphorescent-sensitized fluorescent white OLEDs (W1) obtained in example 1 of the present invention.
FIG. 5 is a schematic view showing the device structure of the phosphorescence-sensitized fluorescent white light OLEDs (W2) according to example 2 of the present invention. Wherein 1 'represents a substrate, 2' represents an anode, 3 'represents a hole injection layer, 4' represents a hole transport layer, 5 'represents an electron blocking layer, 6' represents a blue light emitting layer, 7 'represents a yellow light emitting layer, 8' represents an electron transport layer, 9 'represents an electron injection layer, and 10' represents a cathode.
FIG. 6 is a graph showing current efficiency, power efficiency and external quantum efficiency-luminance characteristics of phosphorescent-sensitized fluorescent OLEDs (W2) obtained in example 2 of the present invention.
FIG. 7 shows that the phosphorescence-sensitized fluorescent white light OLEDs (W2) obtained in example 2 of the present invention are 1000cd/m2、3000cd/m2And 5000cd/m2Electroluminescence spectrum at brightness.
FIG. 8 is a graph showing current density-luminance-voltage characteristics of phosphorescent-sensitized fluorescent white OLEDs (W2) obtained in example 2 of the present invention.
Detailed Description
The present invention will be described in further detail with reference to examples and drawings, but the present invention is not limited thereto.
Example 1
A schematic structural diagram of the phosphorescence-sensitized fluorescent white light OLEDs (W1) of this example is shown in FIG. 1. Firstly, carrying out ultrasonic treatment on ITO conductive glass for 60 minutes by using an alkaline cleaning agent, then rubbing and washing the ITO conductive glass by using tap water, washing the ITO conductive glass by using deionized water, drying the residual water by using high-pressure nitrogen, then baking the ITO conductive glass in an oven at 120 ℃ for 30 minutes, then treating the surface of the ITO conductive glass by using ultraviolet ozone for 6 minutes, putting the ITO conductive glass into a film coating machine, vacuumizing by using a molecular pump, and when the surface of the film coating machine is used, cleaning the ITO conductive glass by using tap water, cleaning the ITO conductive glass byPressure below 8 x 10-5And (Pa), sequentially evaporating the thin films on the ITO conductive glass. Firstly, evaporating a hole injection layer material HAT-CN on the surface of the ITO conductive glass, and controlling the evaporation rate at
The thickness was 15 nm. Then sequentially evaporating a hole transport layer material TAPC (thermal insulation coating), wherein the evaporation rate is controlled at
The thickness is 60 nm; the electron barrier material TCTA with evaporation rate controlled in
The thickness is 10 nm; host material 26DCzPPy of yellow light emitting layer and doped yellow phosphorescent sensitizer Ir (ppy)3(6 wt.%) and yellow fluorescent luminescent material TBRb (2 wt.%), the evaporation rate is
And
the thickness of the yellow light-emitting layer is 5 nm; blue light emitting layer host material 26DCzPPy and doped blue light phosphorescence sensitizer fac-Ir (iprmi)3(8 wt.%) and blue-light fluorescent luminescent material TBPe (1 wt.%), the evaporation rate is in turn
And
the thickness of the blue light emitting layer is 15 nm; the electron transport layer material TmPyPB, the evaporation rate is controlled at
The thickness is 45 nm; the material LiF of the electron injection layer is controlled in the evaporation rate
The thickness was 1 nm.Finally, evaporating a cathode material Al, and controlling the evaporation rate at
The thickness was 100 nm. The speed and the thickness of each functional layer of vapor plating are controlled by a quartz crystal oscillator film thickness detector, and the obtained white light OLEDs device has the following structure: ITO/HAT-CN (15nm)/TAPC (60nm)/TCTA (10nm)/26DCzPPy 6 wt.% Ir (ppy)3:2wt.％TBRb(5nm)/26DCzPPy:8wt.％fac-Ir(iprpmi)3:1wt.％TBPe(15nm)/TmPyPB(45nm)/LiF(1nm)/Al(100nm)。
The current efficiency, power efficiency and external quantum efficiency-luminance characteristic curve, electroluminescence spectrogram and current density-luminance-voltage characteristic curve of the phosphorescence-sensitized fluorescent white light device W1 obtained in the implementation are respectively shown in FIG. 2, FIG. 3 and FIG. 4.
Example 2
A schematic structural diagram of the phosphorescence-sensitized fluorescent white light OLEDs (W2) of this example is shown in FIG. 5. Firstly, carrying out ultrasonic treatment on ITO conductive glass for 60 minutes by using an alkaline cleaning agent, then rubbing and washing the ITO conductive glass by using tap water, washing the ITO conductive glass by using deionized water, drying the residual water by using high-pressure nitrogen, then placing the ITO conductive glass into an oven at 120 ℃ for baking for 30 minutes, then placing the ITO conductive glass into a film coating machine after the surface of the ITO conductive glass is treated by using ultraviolet ozone for 6 minutes, vacuumizing by using a molecular pump, and when the pressure intensity of the film coating machine is lower than 8 multiplied by 10-5And (Pa), sequentially evaporating the thin films on the ITO conductive glass. Firstly, evaporating a hole injection layer material HAT-CN on the surface of the ITO conductive glass, and controlling the evaporation rate at
The thickness was 15 nm. Then sequentially evaporating a hole transport layer material TAPC (thermal insulation coating), wherein the evaporation rate is controlled at
The thickness is 60 nm; the electron barrier material TCTA with evaporation rate controlled in
The thickness is 10 nm; blue light emissionLayer host material 26DCzPPy and doped blue phosphorescent sensitizer fac-Ir (iprmi)3(8 wt.%) and blue-light fluorescent luminescent material TBPe (1 wt.%), the evaporation rate is in turn
And
the thickness of the blue light emitting layer is 3 nm; host material 26DCzPPy of yellow light emitting layer and doped yellow phosphorescent sensitizer Ir (ppy)3(6 wt.%) and yellow fluorescent luminescent material TBRb (2 wt.%), the evaporation rate is
And
the thickness of the yellow light-emitting layer is 15 nm; the electron transport layer material TmPyPB, the evaporation rate is controlled at
The thickness is 45 nm; the material LiF of the electron injection layer is controlled in the evaporation rate
The thickness was 1 nm. Finally, evaporating a cathode material Al, and controlling the evaporation rate at
The thickness was 100 nm. The speed and the thickness of each functional layer of vapor plating are controlled by a quartz crystal oscillator film thickness detector, and the obtained white light OLEDs device has the following structure: ITO/HAT-CN (15nm)/TAPC (60nm)/TCTA (10nm)/26DCzPPy 8 wt.% fac-Ir (iprmi)3:1wt.％TBPe(3nm)/26DCzPPy:6wt.％Ir(ppy)3:2wt.％TBRb(15nm)/TmPyPB(45nm)/LiF(1nm)/Al(100nm)。
The current efficiency, power efficiency and external quantum efficiency-luminance characteristic curve, electroluminescence spectrum and current density-luminance-voltage characteristic curve of the phosphorescent-sensitized fluorescent device W2 obtained in this example are shown in fig. 6,7 and 8, respectively.
As can be seen from fig. 2,3, 4, 6,7 and 8, by adopting the phosphor-sensitized fluorescence, the positions and thicknesses of the blue light emitting layer and the yellow light emitting layer can be designed to produce the all-fluorescent white OLEDs with high efficiency, low roll-off and stable spectrum. From the electroluminescence spectra, both the device W1 and the device W2 exhibited emission peaks of blue fluorescence TBPe and yellow fluorescence TBRb, and the electroluminescence spectra of both devices were 1000cd/m2To 5000cd/m2Is very stable under the brightness, and realizes good white light emission. The maximum current efficiency, power efficiency and external quantum efficiency obtained by the devices W1 and W2 were 27.5cd/A, 25.8lm/W, 10.3% and 42.4cd/A, 36.4lm/W, 14.3%, and 1000cd/m2Still at 25.8cd/a, 15.0lm/W, 9.5% and 34.0cd/a, 19.8lm/W, 11.6% luminance, both devices showed high efficiency characteristics while the efficiency roll-off at high luminance was also well improved. The phosphorescence-sensitized fluorescence method adopted by the invention is proved to have the excellent performance of preparing the high-efficiency low-roll-off all-fluorescence white light OLEDs, and has potential application prospect.
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such changes, modifications, substitutions, combinations, and simplifications are intended to be included in the scope of the present invention.
Claims (10)
1. A phosphorescence-sensitized fluorescent white light organic light-emitting diode is characterized in that: the structure sequentially comprises a substrate, an anode, a hole injection layer, a hole transport layer, an electron blocking layer, a light emitting layer, an electron transport layer, an electron injection layer and a cathode; the light-emitting layer is formed by combining a blue light-emitting layer and a yellow light-emitting layer, the blue light-emitting layer is formed by doping a blue light phosphorescence sensitizer and a blue light fluorescence object in a host material, and the yellow light-emitting layer is formed by doping a yellow light phosphorescence sensitizer and a yellow light fluorescence object in the host material.
2. The phosphor-sensitized fluorescent white light organic light emitting diode according to claim 1, wherein: the host material of the blue light emitting layer is 26DCzPPy, and the blue light phosphorescence sensitizer is fac-Ir (iprami)3The blue light fluorescent guest is TBPe; the host material of the yellow light emitting layer is 26DCzPPy, and the yellow phosphorescent sensitizer is Ir (ppy)3The yellow fluorescent guest is TBRb.
3. The phosphor-sensitized fluorescent white light organic light emitting diode according to claim 2, wherein: the blue light phosphorescence sensitizer fac-Ir (iprmi)3The doping concentration of the blue light fluorescent guest TBPe is 8 wt.%, and the doping concentration of the blue light fluorescent guest TBPe is 1 wt.%; the yellow phosphorescent sensitizer Ir (ppy)3Has a doping concentration of 6 wt.%, and the yellow fluorescent guest TBRb has a doping concentration of 2 wt.%.
4. The phosphor-sensitized fluorescent white light organic light emitting diode according to claim 3, wherein: the thickness of the blue light emitting layer is 3-15 nanometers, and the thickness of the yellow light emitting layer is 5-15 nanometers.
5. The phosphorescence-sensitized fluorescent white light organic light-emitting diode according to any one of claims 1 to 4, wherein: the substrate is one of glass, quartz or flexible plastic; the anode is one of ITO, ZnO, FTO or graphene.
6. The phosphorescence-sensitized fluorescent white light organic light-emitting diode according to any one of claims 1 to 4, wherein: the hole injection layer adopts an organic material HAT-CN or an inorganic material MoO3、WO3Or V2O5One of (1); the hole transport layer is TAPC; the electron blocking layer is TCTA.
7. The phosphorescence-sensitized fluorescent white light organic light-emitting diode according to any one of claims 1 to 4, wherein:the electron transport layer is TmPyPB; the electron injection layer adopts LiF, Liq and Li2CO3Or Cs2CO3One kind of (1).
8. The phosphorescence-sensitized fluorescent white light organic light-emitting diode according to any one of claims 1 to 4, wherein: the cathode is selected from one of gold, silver, aluminum or silver-magnesium alloy.
9. The phosphorescence-sensitized fluorescent white light organic light-emitting diode according to any one of claims 1 to 4, wherein: the thickness of the hole injection layer is 5-20 nanometers, the thickness of the hole transmission layer is 50-90 nanometers, the thickness of the electron blocking layer is 5-15 nanometers, the thickness of the light emitting layer is 15-30 nanometers, the thickness of the electron transmission layer is 40-80 nanometers, the thickness of the electron injection layer is 1-5 nanometers, and the thickness of the cathode is 100-200 nanometers.
10. The method for preparing a phosphorescence-sensitized fluorescent white light organic light-emitting diode according to any one of claims 1 to 9, characterized by comprising the steps of: firstly, carrying out ultrasonic treatment, deionized water flushing, nitrogen blow-drying, baking in a 120 ℃ oven, carrying out ultraviolet ozone treatment on the surface of the ITO glass, then putting the ITO glass into a vacuum coating machine, and vacuumizing by using a molecular pump until the pressure is 8 multiplied by 10-5And after the light emitting diode is below Pa, sequentially evaporating a hole injection layer, a hole transport layer, an electron blocking layer, a light emitting layer, an electron transport layer, an electron injection layer and a cathode to obtain the phosphorescence-sensitized fluorescent white light organic light emitting diode.
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